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Two-dimensional materials and their heterostructures constitute a promising platform to study correlated electronic states, as well as the many-body physics of excitons. Transport measurements on twisted graphene bilayers have revealed a plethora of intertwined electronic phases, including Mott insulators, strange metals and superconductors 1 – 5 . However, signatures of such strong electronic correlations in optical spectroscopy have hitherto remained unexplored. Here we present experiments showing how excitons that are dynamically screened by itinerant electrons to form exciton-polarons 6 , 7 can be used as a spectroscopic tool to investigate interaction-induced incompressible states of electrons. We study a molybdenum diselenide/hexagonal boron nitride/molybdenum diselenide heterostructure that exhibits a long-period moiré superlattice, as evidenced by coherent hole-tunnelling-mediated avoided crossings of an intralayer exciton with three interlayer exciton resonances separated by about five millielectronvolts. For electron densities corresponding to half-filling of the lowest moiré subband, we observe strong layer pseudospin paramagnetism, demonstrated by an abrupt transfer of all the (roughly 1,500) electrons from one molybdenum diselenide layer to the other on application of a small perpendicular electric field. Remarkably, the electronic state at half-filling of each molybdenum diselenide layer is resilient towards charge redistribution by the applied electric field, demonstrating an incompressible Mott-like state of electrons. Our experiments demonstrate that optical spectroscopy provides a powerful tool for investigating strongly correlated electron physics in the bulk and paves the way for investigating Bose–Fermi mixtures of degenerate electrons and dipolar excitons. Optical spectroscopy is used to probe correlated electronic states in a moiré heterostructure, showing many-body effects such as strong layer paramagnetism and an incompressible Mott-like state of electrons.

A Bose–Einstein condensate is the ground state of a dilute gas of bosons, such as atoms cooled to temperatures close to absolute zero 1 . With much smaller mass, excitons (bound electron–hole pairs) are expected to condense at considerably higher temperatures 2 – 7 . Two-dimensional van der Waals semiconductors with very strong exciton binding are ideal systems for the study of high-temperature exciton condensation. Here we study electrically generated interlayer excitons in MoSe 2 –WSe 2 atomic double layers with a density of up to 10 12 excitons per square centimetre. The interlayer tunnelling current depends only on the exciton density, which is indicative of correlated electron–hole pair tunnelling 8 . Strong electroluminescence arises when a hole tunnels from WSe 2 to recombine with an electron in MoSe 2 . We observe a critical threshold dependence of the electroluminescence intensity on exciton density, accompanied by super-Poissonian photon statistics near the threshold, and a large electroluminescence enhancement with a narrow peak at equal electron and hole densities. The phenomenon persists above 100 kelvin, which is consistent with the predicted critical condensation temperature 9 – 12 . Our study provides evidence for interlayer exciton condensation in two-dimensional atomic double layers and opens up opportunities for exploring condensate-based optoelectronics and exciton-mediated high-temperature superconductivity 13 . Condensation of interlayer excitons at temperatures above 100 kelvin is demonstrated in a van der Waals heterostructure consisting of two-dimensional atomic double layers of transition metal chalcogenides.

Many linked processes occur concurrently in strongly excited semiconductors, such as interband and intraband absorption, scattering of electrons and holes by the heated lattice, Pauli blocking, bandgap renormalization and the formation of Mahan excitons. In this work, we disentangle their dynamics and contributions to the optical response of a ZnO thin film. Using broadband pump-probe ellipsometry, we can directly and unambiguously obtain the real and imaginary part of the transient dielectric function which we compare with first-principles simulations. We find interband and excitonic absorption partially blocked and screened by the photo-excited electron occupation of the conduction band and hole occupation of the valence band (absorption bleaching). Exciton absorption turns spectrally narrower upon pumping and sustains the Mott transition, indicating Mahan excitons. Simultaneously, intra-valence-band transitions occur at sub-picosecond time scales after holes scatter to the edge of the Brillouin zone. Our results pave new ways for the understanding of non-equilibrium charge-carrier dynamics in materials by reliably distinguishing between changes in absorption coefficient and refractive index, thereby separating competing processes. This information will help to overcome the limitations of materials for high-power optical devices that owe their properties from dynamics in the ultrafast regime.

Silicon dominates contemporary solar cell technologies 1 . But when absorbing photons, silicon (like other semiconductors) wastes energy in excess of its bandgap 2 . Reducing these thermalization losses and enabling better sensitivity to light is possible by sensitizing the silicon solar cell using singlet exciton fission, in which two excited states with triplet spin character (triplet excitons) are generated from a photoexcited state of higher energy with singlet spin character (a singlet exciton) 3 – 5 . Singlet exciton fission in the molecular semiconductor tetracene is known to generate triplet excitons that are energetically matched to the silicon bandgap 6 – 8 . When the triplet excitons are transferred to silicon they create additional electron–hole pairs, promising to increase cell efficiencies from the single-junction limit of 29 per cent to as high as 35 per cent 9 . Here we reduce the thickness of the protective hafnium oxynitride layer at the surface of a silicon solar cell to just eight angstroms, using electric-field-effect passivation to enable the efficient energy transfer of the triplet excitons formed in the tetracene. The maximum combined yield of the fission in tetracene and the energy transfer to silicon is around 133 per cent, establishing the potential of singlet exciton fission to increase the efficiencies of silicon solar cells and reduce the cost of the energy that they generate. A silicon and tetracene solar cell employing singlet fission uses an eight-angstrom-thick hafnium oxynitride interlayer to promote efficient triplet transfer, increasing the efficiency of the cell.

The fundamental properties of an exciton are determined by the spin, valley, energy, and spatial wavefunctions of the Coulomb-bound electron and hole. In van der Waals materials, these attributes can be widely engineered through layer stacking configuration to create highly tunable interlayer excitons with static out-of-plane electric dipoles, at the expense of the strength of the oscillating in-plane dipole responsible for light-matter coupling. Here we show that interlayer excitons in bi- and tri-layer 2H-MoSe 2 crystals exhibit electric-field-driven coupling with the ground (1 s ) and excited states (2 s ) of the intralayer A excitons. We demonstrate that the hybrid states of these distinct exciton species provide strong oscillator strength, large permanent dipoles (up to 0.73 ± 0.01 enm), high energy tunability (up to ~200 meV), and full control of the spin and valley characteristics such that the exciton g-factor can be manipulated over a large range (from −4 to +14). Further, we observe the bi- and tri-layer excited state (2 s ) interlayer excitons and their coupling with the intralayer excitons states (1 s and 2 s ). Our results, in good agreement with a coupled oscillator model with spin (layer)-selectivity and beyond standard density functional theory calculations, promote multilayer 2H-MoSe 2 as a highly tunable platform to explore exciton-exciton interactions with strong light-matter interactions. Here, the authors discover the ground and excited state interlayer excitons in bi- and tri-layer 2H-MoSe 2 crystals which exhibit electric-field-driven hybridisation with the intralayer A excitons, showing distinct spin, layer and valley characteristics.

Defects in conventional semiconductors substantially lower the photoluminescence (PL) quantum yield (QY), a key metric of optoelectronic performance that directly dictates the maximum device efficiency. Two-dimensional transition-metal dichalcogenides (TMDCs), such as monolayer MoS₂, often exhibit low PL QY for as-processed samples, which has typically been attributed to a large native defect density. We show that the PL QY of as-processed MoS₂ and WS₂ monolayers reaches near-unity when they are made intrinsic through electrostatic doping, without any chemical passivation. Surprisingly, neutral exciton recombination is entirely radiative even in the presence of a high native defect density. This finding enables TMDC monolayers for optoelectronic device applications as the stringent requirement of low defect density is eased.

Photodetectors and solar cells based on materials with strongly bound excitons rely crucially on field-assisted exciton ionization. We study the ionization process in multilayer transition-metal dichalcogenides (TMDs) within the Mott-Wannier model incorporating fully the pronounced anisotropy of these materials. Using complex scaling, we show that the field-dependence of the ionization process is strongly dependent on orientation. Also, we find that direct and indirect excitons behave qualitatively differently as a result of opposite effective anisotropy of these states. Based on first-principles material parameters, an analysis of several important TMDs reveals WSe2 and MoSe2 to be superior for applications relying on ionization of direct and indirect excitons, respectively.